Light-driven H2O2 production over redox-active imine-linked covalent organic frameworks

Advanced Powder Materials Pub Date : 2024-01-24 DOI:10.1016/j.apmate.2024.100179

Songlin Zhang, Jinwen Hu, Wenzhe Shang, Jingya Guo, Xusheng Cheng, Suchan Song, Tianna Liu, Wei Liu, Yantao Shi

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Abstract

Imine-linked covalent organic frameworks (COFs) provide distinctive prospects for promoting photocatalytic H₂O₂ production, yet the intricate involvement of imine-derived linkages chemistry under light irradiation remains incompletely elucidated. Here, imine-linked COF-LZU1 demonstrates a visible light-driven H₂O₂ evolution rate of 387 μmol g⁻¹ h⁻¹, particularly, negligible dependence on the sacrificial agents. By virtue of electron paramagnetic spectroscopy and solid-state nuclear magnetic resonance, we experimentally tracked the structure evolution and identified its autooxidation to Wurster's salt mimics under the photocatalytic conditioning. This finding coincides with the radical anion ·O₂⁻ governed reaction pathway and is further rationalized with additional theoretical calculations. This study provides insights into both photophysical/photochemical aspects over the imine-linkage structure.

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在氧化还原活性亚胺连接共价有机框架上产生光驱动的 H2O2

亚胺连接的共价有机框架（COFs）为促进光催化产生 H2O2 提供了独特的前景，但在光照射下亚胺衍生连接化学的复杂参与仍未完全阐明。在这里，亚胺连接的 COF-LZU1 在可见光驱动下的 H2O2 演化率为 387 μmol g-1 h-1，尤其是对牺牲剂的依赖性可以忽略不计。通过电子顺磁谱和固态核磁共振，我们在实验中跟踪了其结构的演变，并确定了其在光催化条件下自氧化成 Wurster 盐模拟物的过程。这一发现与自由基阴离子 -O2- 主导的反应途径相吻合，并通过更多的理论计算得到了进一步的合理解释。这项研究为亚胺连接结构的光物理/光化学方面提供了见解。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Advanced Powder Materials

CiteScore

33.30

自引率

0.00%

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